醋酸混合溶剂中碘催化甲烷部分氧化过程研究

Methane Partial Oxidation Catalyzed by I_2 in Acetic Acid Solution

在醋酸和杂多酸混和溶剂中进行了甲烷液相部分氧化过程研究。进行了碘系列催化剂以及溶剂体系中杂多酸筛选,考察了催化剂用量、磷钨酸浓度、氧化剂类型、反应温度、压力等条件对甲烷转化的影响。结果表明,在磷钨酸浓度0.072 mol/L,碘含量0.04 mol/L,KMnO_4为0.158 mol/L,温度210℃,压力4.0 MPa条件下,甲烷转化率可达12.98%,目的产物醋酸甲酯选择性84.39%。初步探讨了醋酸和磷钨酸混合溶剂中碘催化甲烷液相选择性氧化的亲电反应机理。

The methane partial oxidation in mixed solution of acetic acid and heteropoly acid was studied. The kinds of iodine series catalyst and phosphotungsticacid were screened. The effects of concentration of I2 and phosphotungsticacid, oxidant types, reaction temperature and pressure on the conversion and selectivity of methanol were also investigated. The methane conversion of 12. 98% and methyl acetate selectivity of 84.39% could be obtained under the conditions of the concentration of I2 0.04 mol/L, phosphotungsticacid 0. 072 mol/L, KMnO4 0. 158 mol/L, reaction temperature 210℃ and pressure of methane 4.0 MPa. The mechanism of reaction in the mixed solution was preliminary discussed.